提高 CO 光转化效率的离子液体和钴单原子。
Improving CO photoconversion with ionic liquid and Co single atoms.
机构信息
Department Key Laboratory of Functional Inorganic Materials Chemistry (Ministry of Education), School of Chemistry and Materials Science, International Joint Research Center and Lab for Catalytic Technology, Heilongjiang University, Harbin, Heilongjiang, 150080, P. R. China.
Department Key Laboratory of Functional Inorganic Materials Chemistry (Ministry of Education), International Joint Research Center for Catalytic Technology, School of Physics, Heilongjiang University, Harbin, 150080, P. R. China.
出版信息
Nat Commun. 2023 Mar 16;14(1):1457. doi: 10.1038/s41467-023-36980-5.
Photocatalytic CO conversion promises an ideal route to store solar energy into chemical bonds. However, sluggish electron kinetics and unfavorable product selectivity remain unresolved challenges. Here, an ionic liquid, 1-ethyl-3-methylimidazolium tetrafluoroborate, and borate-anchored Co single atoms were separately loaded on ultrathin g-CN nanosheets. The optimized nanocomposite photocatalyst produces CO and CH from CO and water under UV-vis light irradiation, exhibiting a 42-fold photoactivity enhancement compared with g-CN and nearly 100% selectivity towards CO reduction. Experimental and theoretical results reveal that the ionic liquid extracts electrons and facilitates CO reduction, whereas Co single atoms trap holes and catalyze water oxidation. More importantly, the maximum electron transfer efficiency for CO photoreduction, as measured with in-situ μs-transient absorption spectroscopy, is found to be 35.3%, owing to the combined effect of the ionic liquid and Co single atoms. This work offers a feasible strategy for efficiently converting CO to valuable chemicals.
光催化 CO 转化有望成为将太阳能储存为化学能的理想途径。然而，电子动力学缓慢和不利的产物选择性仍然是未解决的挑战。在这里，将离子液体 1-乙基-3-甲基咪唑四氟硼酸盐和硼酸盐锚定的 Co 单原子分别负载在超薄 g-CN 纳米片上。优化后的纳米复合材料光催化剂在紫外可见光照射下可将 CO 和水转化为 CO 和 CH，与 g-CN 相比，其光活性提高了 42 倍，对 CO 还原的选择性接近 100%。实验和理论结果表明，离子液体提取电子并促进 CO 还原，而 Co 单原子捕获空穴并催化水氧化。更重要的是，通过原位 μs 瞬态吸收光谱测量，发现 CO 光还原的最大电子转移效率为 35.3%，这归因于离子液体和 Co 单原子的协同作用。这项工作为高效将 CO 转化为有价值的化学品提供了一种可行的策略。
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